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However, the synergistic design of SAMs that simultaneously optimizes electronic structure, molecular packing, perovskite crystallization, and interfacial contact remains underexplored, and the development of new SAMs is often impeded by complex synthetic routes. Herein, we developed an asymmetric [1]benzothieno[3,2\u2010b]indole (BTI) core via a concise Fischer indole synthesis. From this core, three SAMs are obtained by sequentially introducing substituents with electron\u2010donating to electron\u2010withdrawing characteristics. As the electron\u2010withdrawing ability of the substituents increases, the SAMs exhibited progressively enhanced electron delocalization, improved energy\u2010level alignment with perovskite, and preserved long\u2010range ordered molecular packing. The improved SAMs film quality enables them to act as effective templating layers for perovskite deposition, directing perovskite crystallization, improving buried interfacial contact, and suppressing interfacial nonradiative recombination. Consequently, the inverted PSCs with F\u20104PABTI deliver a champion power conversion efficiency (PCE) of 26.76%, a high open\u2010circuit voltage (\n                    <jats:italic>V<\/jats:italic>\n                    <jats:sub>OC<\/jats:sub>\n                    ) of 1.203\u00a0V, and markedly improved operational stability. Notably, the large area device (1 cm\n                    <jats:sup>2<\/jats:sup>\n                    ), module (655.2 cm\n                    <jats:sup>2<\/jats:sup>\n                    ), and wide\u2010bandgap device (1.84\u00a0eV) achieve excellent PCEs of 25.38%, 20.59%, and 17.87%, respectively. This work offers a rational molecular design strategy for advancing high\u2010performance and stable PSCs.\n                  <\/jats:p>","DOI":"10.1002\/anie.1678852","type":"journal-article","created":{"date-parts":[[2026,7,30]],"date-time":"2026-07-30T16:11:17Z","timestamp":1785427877000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":1,"title":["Molecular Tailoring of Self\u2010Assembled Monolayers Derived From Asymmetric Benzothienoindole for Efficient and Stable Inverted Perovskite Solar Cells and Modules"],"prefix":"10.1002","volume":"65","author":[{"given":"Shen","family":"Zhong","sequence":"first","affiliation":[{"name":"College of Chemistry and Materials\/Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education\/National Engineering Research Center for Carbohydrate Synthesis, Jiangxi Normal University  Nanchang P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yonglong","family":"Yang","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials\/Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education\/National Engineering Research Center for Carbohydrate Synthesis, Jiangxi Normal University  Nanchang P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zhaojin","family":"Wang","sequence":"additional","affiliation":[{"name":"Faculty of Materials Science and Energy Engineering Shenzhen University of Advanced Technology  Shenzhen China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Gang","family":"Xie","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials\/Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education\/National Engineering Research Center for Carbohydrate Synthesis, Jiangxi Normal University  Nanchang P. R. 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China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Fanyu","family":"Zeng","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials\/Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education\/National Engineering Research Center for Carbohydrate Synthesis, Jiangxi Normal University  Nanchang P. R. China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5435-1744","authenticated-orcid":false,"given":"Zengqi","family":"Huang","sequence":"additional","affiliation":[{"name":"College of Chemistry and Materials\/Key Laboratory of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education\/National Engineering Research Center for Carbohydrate Synthesis, Jiangxi Normal University  Nanchang P. R. 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